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Fourier Transform Infrared Spectroscopy for the Measurement of Spectral Line Profiles

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Fourier Transform Infrared Spectroscopy for the Measurement of Spectral Line Profiles 4 Fourier Transform Infrared Spectroscopy for the Measurement of Spectral Line Profiles Hassen Aroui1, Johannes Orphal2 and Fridolin Kwabia Tchana3 1Laboratoire de Dynamique Moléculaire et Matériaux Photoniques, Université de Tunis, Ecole Supérieure des Sciences et Techniques de Tunis, 2Institute for Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology (KIT), 3Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA), UMR CNRS 7583 Universités Paris Est Créteil et Paris- Diderot, Institut Pierre Simon Laplace, 1Tunisia 2Germany 3France 1. Introduction Our knowledge of the process of global change in Earth's atmosphere is primarily based on experimental observations made in situ or by remote-sensing. The data obtained reveal the state of the atmosphere and provide input data for validation of theoretical models of the atmosphere. In this context, high resolution molecular spectroscopy plays a key role as it is at the heart of optical remote sensing measurements. In fact, infrared spectroscopy is a powerful tool to identify and quantify atmospheric trace species, through the use of characteristic spectral signatures of the different molecular species and their associated vibration-rotation bands in the mid- or near-infrared. Different methods, based on quantitative spectroscopy, permit tropospheric or stratospheric measurements: in situ long path absorption, atmospheric absorption/emission by Fourier transform spectroscopy with high spectral resolution instruments on the ground, airborne, balloon-borne or satellite- borne measurements (Camy-Peyret et al., 2001). In all cases, the quality of the analysis and interpretation of atmospheric spectra requires reference spectroscopic information (positions, intensities, broadenings, profiles…) measured in the laboratory. Such information exists and is compiled in databases such as HITRAN, GEISA and ATMOS, available to the international scientific community. Fourier Transform Infrared (FTIR) can be utilized to measure some components of an unknown mixture and is currently applied to the analysis of solids, liquids, and gases. The term FTIR refers to the manner in which the data is collected and converted from an interference pattern to a spectrum. Fourier transform spectrometers have progressively replaced dispersive instruments for most applications due to their superior speed and sensitivity. They have greatly extended www.intechopen.com 70 Fourier Transform – Materials Analysis the capabilities of infrared spectroscopy and have been applied to many fields that are very difficult or nearly impossible to study by dispersive instruments. Instead of analyzing each spectral component sequentially, as in a dispersive IR spectrometer, all frequencies are examined simultaneously in FTIR spectroscopy. By interpreting the infrared absorption spectrum, information about the structure and the nature of the chemical bonds in a molecule can be determined. For most common materials, the spectrum of an unknown mixture can be identified by comparison to a library of known compounds. The FTIR technique is a powerful tool for identification of chemical species and their structures, for interpretation of the atmospheric spectra by producing an infrared absorption spectrum that is like a molecular fingerprint. This technique can be used to identify chemicals from spills, paints, polymers, coatings, drugs, and contaminants. It can measure more than 120 gaseous pollutants in the ambient air (U.S. Environmental Protection Agency, 2011), such as carbon monoxide, sulfur dioxide, ozone, and many others. This technique can also quantify toxic organic pollutants, such as toluene, benzene, methanol etc. This quantification is based on the fact that every gas has its own specific spectrum. The FTIR sensor monitors the entire infrared spectrum and reads the different fingerprints of the gases present in the atmosphere. FTIR spectroscopy is also extensively used in the study of absorption line profiles to determine spectroscopic parameters related to line broadening. This chapter describes laboratory measurements of line parameters for atmospheric trace species, using Fourier transform spectroscopy in the infrared spectral range. An illustration is given with the example of atmospheric molecules such as NH3, OCS and CH3Br, for which we have determined line intensities, self- and foreign-gas broadening coefficients, pressure-induced line shifts, as well as line-mixing coefficients for these molecules for more than 300 rovibrational lines located in the spectral range 1000-3000 cm-1, at room and low temperatures. A non-linear least-squares multi-spectrum fitting procedure, including Doppler, and line- mixing effects, has been used to retrieve line parameters from more than twenty experimental spectra, recorded at different pressures of the molecules. The accuracies of the results are also estimated and discussed as a function of the measured parameter. The results, obtained for several branches of the molecules considered here, will be presented and analyzed as a function of gas pressure, temperature, rotational quantum numbers and vibrational bands. From the intensity measurements, we have determined effective transition dipole moments, vibrational band strengths as well as Herman–Wallis parameters for some bands taking into account Coriolis and l-type interactions. For the NH3 molecule, the results concerning line-mixing demonstrate a large amount of coupling between the symmetric and asymmetric components of inversion doublets. The pressure shift coefficients and line-mixing parameters are both positive and negative. Some groups of lines illustrate a correlation between line-mixing and line shift phenomena, demonstrated by a nonlinear pressure dependence of the line position. www.intechopen.com Fourier Transform Infrared Spectroscopy for the Measurement of Spectral Line Profiles 71 Excluding the Introduction and the Conclusion, this chapter is divided into three sections. The FTIR spectroscopy technique is described in detail in section 2. In particular, the model used to describe the instrument line shape function of the Fourier transform spectrometer is presented. Measurement of line profiles using Fourier transform spectroscopy is presented in section 3. In this section, the measured broadening and shift coefficients, as well as line intensities and line-mixing parameters are presented and discussed. The rotational dependence of the pressure broadening coefficients is fitted using empirical polynomial equations to provide empirical interpolation and extrapolation models. 2. Fourier transform spectroscopy 2.1 Quantitative absorption spectroscopy Infrared spectroscopy is the absorption measurement of different IR frequencies by a sample located in the path of an IR beam. Using various sampling accessories, the spectrometers can accept a wide range of sample types such as gases, liquids, and solids. The basic principle for the evaluation in IR spectroscopy is the Beer-Lambert law which was defined in 1852. This law relates the absorption of light to the properties of the material through which the light is traveling. Absorption spectroscopy consists of the application of this law which illustrates that when traversing a measurement cell, the light intensity decreases exponentially: I=I0 ()exp{ -α()`} , (1) where α(σ) (in cm-1) is the absorption coefficient of the material, σ is the wavenumber (in cm-1), ` is the absorption path length (in cm). I0(σ) and I(σ) are the intensity of a collimated light beam (in Wm-2) respectively before and after absorption by the sample. The transmission spectrum T(σ) is the ratio of I(σ) by I0(σ): I() T()= . (2) I(0 ) Eq. (1) can be expressed as a function of the absorption cross section σe(σ) (in cm-2 molecule-1). I=I0e ()exp{ - ()N`} . (3) N is the particle density (in molecule cm-3). At standard conditions of pressure (P = 1 atm) and the temperature (T = 273.15 K), N is equal to the Loschmidt number1 (Auwera, 2004): nL = 2.6867661 (47) x 1019 molecule cm-3 atm-1. 1 Computed from the value of the molar gas constant R available in February 2003 on the website of the Physics Laboratory of the National Institute of Science and Technology (http://physics.nist.gov/). www.intechopen.com 72 Fourier Transform – Materials Analysis 2.2 Fourier transform spectroscopy 2.2.1 Introduction Since the invention of the first spectrophotometers in the beginning of 20th century, a rapid technological progress has occurred. The first-generation spectrometers were all dispersive with a prism or grating as dispersive elements. In the mid 1960s infrared spectroscopy has seen the advent of the Fourier transform spectrometer. These second-generation infrared spectrometers have significant advantages compared to dispersive spectrometers. 2.2.2 General description The basic experimental set up of the Fourier transform spectrometer is constituted by the Michelson interferometer. As shown in Fig. 1, light from a source (S) is collimated and then divided at a beam splitter (L) into two beams of equal amplitude. These beams are reflected back on themselves by two separate mirrors, one fixed (M2) and the other movable (M1). Each single beam strikes the beam splitter again, where they are recombined and directed to the detector (D). The two components in the recombined beam interfere with each other and form a spot whose intensity depends upon the different paths traversed by the two beams before recombination. As one mirror moves, the path length of one beam changes and the spot
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